EP1229599A2 - Verfahren zur Hestellung von gesintertem Substrat für alkalische Speicherbatterie - Google Patents

Verfahren zur Hestellung von gesintertem Substrat für alkalische Speicherbatterie Download PDF

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Publication number
EP1229599A2
EP1229599A2 EP02002290A EP02002290A EP1229599A2 EP 1229599 A2 EP1229599 A2 EP 1229599A2 EP 02002290 A EP02002290 A EP 02002290A EP 02002290 A EP02002290 A EP 02002290A EP 1229599 A2 EP1229599 A2 EP 1229599A2
Authority
EP
European Patent Office
Prior art keywords
nickel
particles
pore former
substrate
sintered
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP02002290A
Other languages
English (en)
French (fr)
Other versions
EP1229599A3 (de
Inventor
Hiroshi Fukuda
Masao Takee
Hideo Kasuga
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sanyo Electric Co Ltd
Original Assignee
Sanyo Electric Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Sanyo Electric Co Ltd filed Critical Sanyo Electric Co Ltd
Publication of EP1229599A2 publication Critical patent/EP1229599A2/de
Publication of EP1229599A3 publication Critical patent/EP1229599A3/de
Withdrawn legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/80—Porous plates, e.g. sintered carriers
    • H01M4/801—Sintered carriers
    • H01M4/803—Sintered carriers of only powdered material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/80—Porous plates, e.g. sintered carriers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
    • B22F3/10—Sintering only
    • B22F3/11—Making porous workpieces or articles
    • B22F3/1121—Making porous workpieces or articles by using decomposable, meltable or sublimatable fillers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
    • B22F3/10—Sintering only
    • B22F3/11—Making porous workpieces or articles
    • B22F3/1121—Making porous workpieces or articles by using decomposable, meltable or sublimatable fillers
    • B22F3/1134—Inorganic fillers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2998/00—Supplementary information concerning processes or compositions relating to powder metallurgy
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T29/00—Metal working
    • Y10T29/10—Battery-grid making
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T29/00—Metal working
    • Y10T29/49—Method of mechanical manufacture
    • Y10T29/49002—Electrical device making
    • Y10T29/49108—Electric battery cell making
    • Y10T29/49115—Electric battery cell making including coating or impregnating

Definitions

  • the present invention relates to a sintered substrate of alkaline batteries and the manufacturing method thereof.
  • sintered substrates As substrate grids for electrodes of alkaline batteries including nickel-hydrogen storage batteries, sintered substrates have been commonly used.
  • a sintered substrate is formed by applying nickel powder to a porous substrate made of nickel or the like, and by sintering the substrate. Among such porous substrates are punched metals and punched nickel plates. By impregnating the sintered substrate with an active material, an electrode can be formed.
  • the production of alkaline batteries having a higher energy density requires an increased amount of impregnated active material, since the operation of a battery is greatly dependent on the active material.
  • sintered substrates have a high porosity and hold a sufficient amount of active material in those pores.
  • porous sintered substrate is attainable by using a punched metal with a reduced thickness or with an increased porosity. Though such methods are considered as valid, some other methods have been developed.
  • a sintered substrate is formed by applying slurry made of nickel powder, water and pore former (hollow resinous particles) to a punched metal.
  • a technique disclosed by the Japanese Patent Laid-Open Application Number S61-185685 in which a sintered substrate is formed by applying a mixture of water and metal-coated pore former particles to a punched metal and then sintering the punched metal together with the mixture.
  • FIG. 3 shows an electrode that uses a sintered substrate formed based on the former technique.
  • the nickel particles (FIG. 3B) and the core (punched metal) are sintered and bonded together to form a nickel framework (FIG. 3A).
  • FIG. 3A shows a nickel framework
  • FIG. 4 shows an electrode that uses a sintered substrate manufactured according to the latter technique.
  • a punched metal and hollow spheric nickel shells (FIG.4B) are sintered together to form a nickel framework (FIG.4A).
  • the nickel shells of this nickel framework (FIG. 4C) have relatively large pores, and they are joined together with some spaces in-between. Though not illustrated here for the sake of convenience, these pores and spaces are filled with an active material.
  • sintered substrates with relatively high porosity.
  • the sintered substrates have a problem of strength.
  • Sintered substrates manufactured by the former technique have a higher porosity, with relatively large pores formed inside the nickel frameworks by the effect of the pore former . But this porous construction can cause brittle failure, including surface detachment and cracking.
  • sintered substrates according to the second technique have pores of an average size generated from metal-plated pore former . But these sintered substrates do not have a sufficient level of strength, and they are weak especially against stress applied from the direction of the thickness. This can cause a problem similar to those with the first technique. Such problems can occur whether the shape of the battery is cylindrical or rectangular.
  • the present invention intends to provide a manufacturing method for producing sintered substrates of alkaline batteries having high porosity and high strength.
  • 'pore former refers to a substance that remains in the form of particles when a first step is completed but disappears during a second step.
  • the pore former includes resinous powder which dissipates when it is burned.
  • pore former is provided in the form of spheric particles having a diameter greater than that of a particle made of nickel or principally made of nickel.
  • the pore former is mixed and knead with the particles that are made of nickel or principally made of nickel, to be arranged almost uniformly in spaces between the nickel particles, so that some of the spaces between them are pressurized and enlarged.
  • the surfaces of the pore former particles are covered with a coating made of nickel or principally made of nickel.
  • the nickel framework is constructed in such a manner that a nickel particle surrounds a nickel shell, and the nickel shell surrounds a relatively large pore. This gives strength and thickness to parts of the nickel framework surrounding relatively large pores, preventing the occurrence of brittle failure. Therefore, even with a higher porosity, the sintered substrate of the present invention can preserve the strength.
  • the sintered substrate of the present invention Compared with sintered substrates manufactured by a conventional manufacturing method which uses non-Ni-coated pore former particles and particles that are made of nickel or principally made of nickel, the sintered substrate of the present invention has high strength. At the same time, the sintered substrate has a greater porosity than sintered substrates manufactured according to a conventional technique which uses only metal-plated pore former particles.
  • FIG. 1 is a perspective view showing a cross-section of a cylindrical alkaline storage battery (a nickel-hydrogen storage battery) that is an embodiment of a sintered substrate manufactured by a method of the present invention.
  • the sintered substrate is used for a positive electrode 1.
  • the alkaline storage battery consists of a set of electrodes 4 and a cylindrical external casing 6 of AA size.
  • the set of electrodes 4, impregnated with an electrolytic solution, is housed in the cylindrical external casing 6.
  • the set of electrodes 4 is formed by spirally winding a positive electrode 1 and a negative electrode 2 with a separator 3 in-between.
  • the negative electrode 2 is formed from a Ni-plated porous Fe substrate (e.g. a punched metal). A paste containing hydrogen-absorbing alloys is applied to the substrate before sintering.
  • the negative electrode 2 is connected by a negative collector 5 to an inner base surface of the external casing 6 which serves as a negative electrode terminal.
  • An opening at the tip of the external casing 6 is closed with a sealing plate 12 via a gasket 11.
  • a positive electrode terminal 13 is inserted to cover a central opening 14 of the sealing plate 12.
  • a valve plate 8 Between the sealing plate 12 and positive electrode terminal 13, there arranged a valve plate 8, a holding plate 9 and a coil spring 10 in this order from the bottom.
  • the valve plate 8 and the holding plate 9 can work as a safety valve when they are pressed, due to the elasticity of the spring 10, against the vicinity of the central opening 14.
  • the positive electrode 1 is joined by a positive collector 7 and the sealing plate 12 with the positive electrode terminal 13.
  • the construction of the positive electrode 1 is described in the following.
  • FIG. 2A shows cross-sections of the positive electrode in this embodiment.
  • the positive electrode 1 is composed of nickel frameworks 100, which uses a punched metal 10 as a porous substrate grid, nickel particles 120 and nickel shells 110 formed on the surface of the punched metal 10.
  • the punched metal 10 is formed by plating a plate-like Fe core with nickel. On the surface of the punched metal 10, there are through holes 101 formed sporadically.
  • the nickel framework 100 is arranged so as to fill in the through holes 101 and to cover the surfaces of the punched metals 10 in a layered form.
  • the nickel framework 100 shows several characteristics that are essential to the manufacturing method of the present invention.
  • the nickel framework 100 of FIG. 2B consists of the nickel particles 120 and the nickel shells 110a that are sintered together.
  • the nickel shell 110a has a relatively large pore (in FIG. 2A and 2B, such relatively large pores are filled with an active material) which is formed in the place of a pore forming particle that disappeared when sintered.
  • the nickel shell 110a that is what used to be a coating on the surface of the pore forming particle.
  • the nickel shell 110a is obtained from a nickel coating formed on the surface of a pore forming particle.
  • the pore former disappears, leaving the nickel shells 110a instead.
  • the pore former particles should preferably be made of a material that dissipates during the sintering step, specifically, from resins. But the pore former can be made from any material on condition that the material, applied on a punched metal, can disappear by means of some processing.
  • nickel framework 100 shows a greater porosity than a conventional nickel framework that is made up only of sintered nickel particles.
  • the nickel framework 100 is constructed in such a manner that the relatively large pores are each surrounded by the nickel shell 110a, and the nickel shell 110a are each surrounded by the nickel particles, and these elements are fusion-bonded. This gives strength and thickness to parts of the nickel framework 100 surrounding the large pores, preventing the occurrence of brittle failure. This makes it possible to produce a sintered substrate having a great porosity without degrading its strength. Therefore, compared with conventional manufacturing methods for producing sintered substrates from non-Ni-coated particles or only from metal-plated pore former particles, the manufacturing method of the present invention can produce a sintered substrate with high strength and high porosity.
  • the sintered substrate is filled with an active material. Any commonly used methods can serve for this purpose, including impregnating.
  • This active material is put in the relatively small spaces 110c of the nickel framework and the relatively large pores 110b (as shown in FIG.2B, the small spaces among the nickel particles 120 are actually filled with the active material), to ensure that a formed positive electrode 1 is filled with a sufficient amount of active material in light of a conventional electrode.
  • the nickel framework of the positive electrode 1 shows much higher strength against a stress applied from the direction of the thickness of the positive electrode 1, as shown in FIG. 2A, than a nickel framework composed merely of nickel shells. Therefore, when such a positive electrode is spirally wound to fit in the cylindrical external casing 6, it is less likely to suffer the formation of cracks on the surface than conventional ones.
  • batteries of superior characteristics can be manufactured.
  • the following describes a manufacturing method for the sintered substrate that is the embodiment of the present invention. As actual examples, a sintered substrate for the positive electrode 1 and slightly modified sintered substrates were prepared. The following also describes sintered substrates of comparative examples.
  • carbonyl nickel powder having an average diameter of 2 ⁇ m and an apparent density of 0.5g/cm 3 was mixed with water and methylcellulose (carbonyl nickel powder-100%, water-100%, methylcellulose-2%, by weight), before adding 10wt% of Ni-coated pore former particles into the mixture.
  • the pore former particles were made of a resin, such as acrylonitrile and methyl methacrylate, and their surfaces were coated with a nickel layer having a thickness of 1 ⁇ m to 5 ⁇ m (specifically, those particles are coated with nickel) .
  • the mixture was then stirred to make slurry.
  • the slurry was applied to the surface of a punched metal, or a Ni-plated Fe core, dried and sintered in a furnace at temperatures ranging from 800°C to 1000°C.
  • the spheric pore former particles are made from solid resinous particles in the actual example 1
  • the spheric pore former particles used for the substrate of actual example 2-A are hollow and coated with nickel (these hollow spaces are filled with a hydrocarbon having a low melting point, such as butane and methane). These hollow pore former particles are used by 8 weight percent for the actual example 2-A. Note that it is possible to make the substrate of the present invention from hollow pore former particles. At the early stage of the sintering process, a hydrocarbon that has a low boiling point and was filled in the hollow spaces disappeared, which facilitated the process of forming pores. Apart from this point, the substrate of this actual example 2-A was the same as the substrate of the actual example 1.
  • the substrate of this actual example 2-B was the same as the substrate of the actual example 2-A, except that it used 10wt% of the Ni-coated hollow spheric pore former particles, as used for the actual example 2-A.
  • the substrate of the actual example 2-C was the same as the substrate of the actual example 2-A, except that it used 12wt% of the Ni-coated hollow spheric pore former particles, as used for the actual example 2-A.
  • the substrate of the actual example 3 was the same as the substrate of the actual example 2-A, except that it used 12wt% of Ni-coated hollow spheric pore former particles that contain 0.01% of P.
  • the substrate of the comparative example 1-A was the same as the substrate of the actual example 2-A, except that it used 3wt% of hollow spheric pore former particles that were not coated with nickel.
  • the substrate of the comparative example 1-B was the same as the substrate of the actual example 2-A, except that it used 4wt% of hollow spheric pore former particles that were not coated with nickel.
  • the substrate of the comparative example 1-C was the same as the substrate of the actual example 2-A, except that it used 5wt% of hollow spheric pore former particles that were not coated with nickel.
  • the substrate of the comparative example 2 was the same as the substrate of the actual example 1, except that it used 60wt% of the Ni-coated hollow spheric pore former particles, as used for the actual example 1.
  • the sintered substrates were soaked in water for one hour.
  • the porosities of the substrates were determined by the amounts of water included.
  • a flat part of a pushpin-like metal was attached to the surface of the sintered substrates with adhesive.
  • the forces (release forces) were measured immediately before the nickel sintered substrates were taken off from the punched metal. These forces represent the strength of the substrates.
  • the substrate of the actual example 3 which uses slurry containing nickel and a small amount of P, has a greater strength than the actual example 2C.
  • P acted as an assisting material in the sintering, which has made the sidereal nickel framework much stronger and thicker.
  • the assisting material is a material that can help reduce a sintering temperature of nickel, including P. But it is more preferable that the assisting material is one of B, In or a combination of them.
  • the effect of the present invention can be achieved whether the shape of the pore former particles contained in the slurry are hollow or solid. Also, it is not affected by how much the Ni-coated pore former particles are contained in the slurry on condition that the amount is within a range of those used for the actual examples. Also, the effect of the present invention will not suffer damage if the assisting material is contained in the pore former particles.
  • the composition ratio at which the particles should be contained can be easily determined through adjustment and testing, to ensure the effect of the present invention.
  • the slurry should preferably have nickel particles and Ni-coated pore former particles at a ratio ranging from 60:40 to 97:3.
  • the sintered substrate should preferably be set within a range from 85% to 92%, so that the substrate has a sufficient active material holding capacity, and at the same time, is made stronger.
  • the Ni-coated pore former particles should preferably have an average diameter ranging from 5 ⁇ m to 70 ⁇ m, and the nickel particles should preferably have an average diameter ranging from 1 ⁇ m to 5 ⁇ m.
  • the present invention can be applied to other alkaline batteries, such as nickel cadmium batteries.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Mechanical Engineering (AREA)
  • Cell Electrode Carriers And Collectors (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Powder Metallurgy (AREA)
EP02002290A 2001-01-31 2002-01-30 Verfahren zur Hestellung von gesintertem Substrat für alkalische Speicherbatterie Withdrawn EP1229599A3 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2001024329 2001-01-31
JP2001024329A JP2002231252A (ja) 2001-01-31 2001-01-31 アルカリ蓄電池用焼結式基板の製造方法

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EP1229599A2 true EP1229599A2 (de) 2002-08-07
EP1229599A3 EP1229599A3 (de) 2003-12-17

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US (1) US6849361B2 (de)
EP (1) EP1229599A3 (de)
JP (1) JP2002231252A (de)
KR (1) KR20020064193A (de)
CN (1) CN1246919C (de)
TW (1) TW541748B (de)

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EP1528613A1 (de) * 2003-10-28 2005-05-04 TDK Corporation Funktionelle, poröse Schicht, Metallschicht und Verfahren zur Herstellung solcher Schichten
EP2865466A1 (de) * 2013-10-22 2015-04-29 Linde Aktiengesellschaft Verfahren zur Modifizierung der Oberflächenstruktur eines Metallkörpers
DE102013226751A1 (de) * 2013-12-19 2015-06-25 Siemens Aktiengesellschaft Verfahren zur Herstellung wenigstens einer Energiespeicherkomponente für einen elektrischen Energiespeicher

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US9446953B2 (en) 2007-07-12 2016-09-20 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Fabrication of metallic hollow nanoparticles
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US20180138110A1 (en) * 2016-11-17 2018-05-17 Texas Instruments Incorporated Enhanced Adhesion by Nanoparticle Layer Having Randomly Configured Voids
US9865527B1 (en) 2016-12-22 2018-01-09 Texas Instruments Incorporated Packaged semiconductor device having nanoparticle adhesion layer patterned into zones of electrical conductance and insulation
US9941194B1 (en) 2017-02-21 2018-04-10 Texas Instruments Incorporated Packaged semiconductor device having patterned conductance dual-material nanoparticle adhesion layer
DE102017110863B4 (de) 2017-05-18 2021-02-04 Zentrum für Sonnenenergie- und Wasserstoff-Forschung Baden-Württemberg Nickelelektrode, Verfahren zu deren Herstellung und deren Verwendung
JP7333300B2 (ja) * 2020-10-26 2023-08-24 プライムプラネットエナジー＆ソリューションズ株式会社 電極の製造方法、電池の製造方法、電極および電池

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Publication number Priority date Publication date Assignee Title
US6849361B2 (en) * 2001-01-31 2005-02-01 Sanyo Electric Co., Ltd. Manufacturing method for sintered substrate of alkaline storage battery
EP1528613A1 (de) * 2003-10-28 2005-05-04 TDK Corporation Funktionelle, poröse Schicht, Metallschicht und Verfahren zur Herstellung solcher Schichten
EP2865466A1 (de) * 2013-10-22 2015-04-29 Linde Aktiengesellschaft Verfahren zur Modifizierung der Oberflächenstruktur eines Metallkörpers
DE102013226751A1 (de) * 2013-12-19 2015-06-25 Siemens Aktiengesellschaft Verfahren zur Herstellung wenigstens einer Energiespeicherkomponente für einen elektrischen Energiespeicher

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CN1369924A (zh) 2002-09-18
US6849361B2 (en) 2005-02-01
US20020150821A1 (en) 2002-10-17
EP1229599A3 (de) 2003-12-17
KR20020064193A (ko) 2002-08-07
JP2002231252A (ja) 2002-08-16
TW541748B (en) 2003-07-11
CN1246919C (zh) 2006-03-22

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